We report a comprehensive first-principles study of the thermodynamics and transport of intrinsic point defects in layered oxide cathode materials LiMO₂ (M = Co, Ni), using density-functional theory and the Heyd–Scuseria–Ernzerhof screened hybrid functional. We find that LiCoO₂ has a complex defect chemistry; different electronic and ionic defects can exist under different synthesis conditions, and LiCoO₂ samples free of cobalt antisite defects can be made under Li-excess (Co-deficient) environments. A defect model for lithium over-stoichiometric LiCoO₂ is also proposed, which involves negatively charged lithium antisites and positively charged small (hole) polarons. In LiNiO₂, a certain amount of Ni³⁺ ions undergo charge disproportionation and the concentration of nickel ions in the lithium layers is high. Tuning the synthesis conditions may reduce the nickel antisites but would not remove the charge disproportionation. In addition, we find that LiMO₂ cannot be doped n- or p-type; the electronic conduction occurs via hopping of small polarons and the ionic conduction occurs via migration of lithium vacancies, either through a monovacancy or divacancy mechanism, depending on the vacancy concentration.